A calibration method for the robotic Tool Center Frame (TCF) was proposed, and a calibration sensor system and experimental platform are constructed in this study. The calibration speed and accuracy of the system were measured and studied. This calibration method involved robot movement along the trajectory of a predetermined circle and a straight line. The photoelectric calibration sensor records the time while the system was moving. The position of the deviation of the tool coordinate system was obtained. In this study the error caused by the photoelectric calibration sensor was analyzed, which may not achieve a rectangular coordinate system due to the cause of the assembly. Experimental results reveal the calibration accuracy of a robot tool coordinate system at ±0.5 mm, and a calibration and recovery time of 15 s. These values meet the requirements for accuracy and efficiency in vehicle production, indicating that our method is capable of calibrating the robot tool coordinate system quickly and effectively.